The Synthesis and Properties of Scandium Coordination Polymer Based on 1,3,5-Benzenetricarboxylic Acid with the Structure of MIL-100

The Synthesis and Properties of Scandium Coordination Polymer Based on 1,3,5-Benzenetricarboxylic Acid with the Structure of MIL-100

Abstract

Metal-Organic Frameworks ï¼ˆMOFsï¼‰ are currently most topical materials for their potential application in gas storage, molecular separation, catalysis, magnetism, etc. The MOF functionalization is essentially important for the application that highly relies on the porosity and stabilities of the MOFs. MIL-100 is regarded as one among the most porous and stable MOFs reported so far. Functionalizing MIL-100 structure with a lighter metal should be available to the gas adsorption ability. As the lightest rare-earth element, scandium can also form theÎ¼3-oxo-centered trinuclear metal cluster, the primary building unit of the MIL-100 structure. Thus, we believe that scandium can also form the giant pore MOF with the MIL-100 structure.Part 1: In the dissertation, scandium trimesate of MIL-100 structure ï¼ˆ1ï¼‰ with formula [Sc3Oï¼ˆOHï¼‰ï¼ˆHï¼‰)2O)+2ï¼ˆBTCï¼‰+2]Â·xH)2OÂ·yDMF ï¼ˆxâ‰ˆ4.5, yâ‰ˆ2.5ï¼‰ was synthesized under solvent thermal condition. The complex was characterized by X-Ray Powder Diffraction, IR spectroscopy, Thermogravimetric analysis, Scanning Electron Microscope and Transmission Electron Microscope. The porosity of the complex 1 was investigated by nitrogen and hydrogen adsorption.Part 2: By depositing Pd nanoparticles on the framework of 1, the post-functionalized porous MOFs of Pd@1 with different Pd concentrations were obtained. They were all characterized by X-ray powder diffraction, SEM, TEM, and nitrogen adsorption studies. The hydrogen storage study on complex 1 and Pd@1 indicates that the Pd insertion decreases the excess adsorption capacity at 77K, but increases the adsorption capacity at 273K. Furthermore, the Pd@1 is applicable for the Pd nanoparticle-catalyzed reaction, demonstrating high catalystic behavior on the cyclohexene reduction to cyclohexane by hydrogen.Part 3: Complexes of 2-3 were synthesized by the reaction of Cdï¼ˆIIï¼‰ ions with imidazole and 2-methylimidazole or 2-nitroimidazole by solvent thermal method. The two complexes were characterized by single-crystal X-ray diffraction, IR spectroscopy, elemental analysis, thermogravimetric analysis. The structural analysis indicated that the complex [Cdï¼ˆim-mimï¼‰2] ï¼ˆ2ï¼‰ crystallized in Orthorhombic, space group P222ï¼ˆ1ï¼‰, a=7.49037ï¼ˆ7ï¼‰ ï¼ˆÂ·ï¼‰,b=7.490 ï¼ˆÂ·ï¼‰,c=15.0169 ï¼ˆÂ·ï¼‰, possessing two-fold interpenetrated diamond-like net; complex [Cdï¼ˆnimï¼‰2] ï¼ˆ3ï¼‰ belonged to Tetragonal space group I4ï¼ˆ1ï¼‰/amd, a=b=6.3904 ï¼ˆ?ï¼‰,c=26.5417 ï¼ˆ?ï¼‰,possessing 2D layer topology net.

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